Uptake of reactive nitrogen on cirrus cloud particles in the upper troposphere and lowermost stratosphere

Kondo, Yutaka; Toon, O. B.; Irie, Hitoshi; Gamblin, B.; Koike, M.; Takegawa, N.; Tolbert, Margaret A.; Hudson, P. K.; Viggiano, Albert A.; Avallone, L. M.; Hallar, A. Gannet; Anderson, B. E.; Sachse, G. W.; Vay, S. A.; Hunton, D. E.; Ballenthin, J. O.; Miller, Thomas M.

doi:10.1029/2002gl016539

Cited by 35 publications

(65 citation statements)

References 18 publications

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“…Observations from recent aircraft campaigns have confirmed laboratory studies indicating HNO 3 uptake by cloud ice (Zondlo et al, 1997;Abbatt, 1997;Kondo et al, 2003;Voigt et al, 2006Voigt et al, , 2007Popp et al, 2007;Scheuer et al, 2010); thus frozen precipitation may play an important role in modulating O 3 production by lightning or aircraft sources of NO x in the upper troposphere. While there are clear differences in the interaction of gas-phase species with ice and liquid water, most models that include scavenging by frozen precipitation do not make any distinction between cold and warm clouds.…”

Section: Introductionsupporting

confidence: 64%

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

2012

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Abstract. Uptake and removal of soluble trace gases and aerosols by precipitation represents a major uncertainty in the processes that control the vertical distribution of atmospheric trace species. Model representations of precipitation scavenging vary greatly in their complexity, and most are divorced from the physics of precipitation formation and transformation. Here, we describe a new large-scale precipitation scavenging algorithm, developed for the UCI chemistrytransport model (UCI-CTM), that represents a step toward a more physical treatment of scavenging through improvements in the formulation of the removal in sub-gridscale cloudy and ambient environments and their overlap within the column as well as ice phase uptake of soluble species. The UCI algorithm doubles the lifetime of HNO 3 in the upper troposphere relative to a scheme with commonly used fractional cloud cover assumptions and ice uptake determined by Henry's Law and provides better agreement with HNO 3 observations. We find that the process of ice phase scavenging of HNO 3 is a critical component of the tropospheric O 3 budget, but that NO x and O 3 mixing ratios are relatively insensitive to large differences in the removal rate. Ozone abundances are much more sensitive to the lifetime of HNO 4 , highlighting the need for better understanding of its interactions with ice and for additional observational constraints.

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Section: Introductionsupporting

confidence: 64%

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

2012

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“…The concentration of the resulting STS population, therefore, would be equivalent to that of the background sulfate aerosol (∼10 cm −3 ) and approximately 10 5 times greater than the particle population reported here. While cirrus ice particles have been observed to contain HNO 3 in the upper troposphere and lower stratosphere (Kondo et al, 2003;) the particles described in this study are unlikely to be composed of ice. Using HNO 3 contents typical of those observed in subtropical cirrus cloud particles , ice particles would need to be at least 50 to 200 µm in diameter to produce an instrument response similar to that shown in Figs.…”

Section: Particle Composition and Sizementioning

confidence: 86%

The observation of nitric acid-containing particles in the tropical lower stratosphere

et al. 2006

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“…High HNO 3 /H 2 O molar ratios in small ice particles (mean radius 5 µm) are found in early cloud stages, decreasing to lower values assuming further ice particles growth. Measurements in young or thin cirrus clouds are rare; in fact, data with particle surface area densities <10 µm 2 cm −3 have been systematically excluded in previous investigations of HNO 3 uptake in cirrus clouds (e.g., Kondo et al, 2003;Ziereis et al, 2004;Popp et al, 2004;Voigt et al, 2006). Hence, our observations combined with microphysical modeling presents a first study of ice particle composition during growth.…”

Section: Discussionmentioning

confidence: 98%

In-situ observations and modeling of small nitric acid-containing ice crystals

Voigt¹,

Kärcher²,

Schläger³

et al. 2007

Atmos. Chem. Phys.

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Abstract. Measurements in nascent ice forming regions are very rare and help understand cirrus cloud formation and the interactions of trace gases with ice crystals. A tenuous cirrus cloud has been probed with in-situ and remote sensing instruments onboard the high altitude research aircraft Geophysica M55 in the tropical upper troposphere. Besides microphysical and optical particle properties, water (H 2 O) and reactive nitrogen species (NO y ) have been measured. In slightly ice supersaturated air between 14.2 and 14.9 km altitude, an unusually low ice water content of 0.031 mg m −3 and small ice crystals with mean radii of 5 µm have been detected. A high nitric acid to water molar ratio (HNO 3 /H 2 O) of 5.4×10 −5 has been observed in the ice crystals, about an order of magnitude higher compared to previous observations in cirrus at temperatures near 202 K. A model describing the trapping of HNO 3 in growing ice particles shows that a high HNO 3 content in ice crystals is expected during early growth stages, mainly originating from uptake in aerosol particles prior to freezing. Water vapor deposition on ice crystals and trapping of additional HNO 3 reduces the molar ratio to values close to the ratio of HNO 3 /H 2 O in the gas phase while the cloud ages.

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Uptake of reactive nitrogen on cirrus cloud particles in the upper troposphere and lowermost stratosphere

Cited by 35 publications

References 18 publications

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone

The observation of nitric acid-containing particles in the tropical lower stratosphere

In-situ observations and modeling of small nitric acid-containing ice crystals

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